KR101012089B1 - Solar cell device comprising a consolidated core/shell polymer-quantum dot composite and preparation thereof - Google Patents
Solar cell device comprising a consolidated core/shell polymer-quantum dot composite and preparation thereof Download PDFInfo
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- KR101012089B1 KR101012089B1 KR1020090043450A KR20090043450A KR101012089B1 KR 101012089 B1 KR101012089 B1 KR 101012089B1 KR 1020090043450 A KR1020090043450 A KR 1020090043450A KR 20090043450 A KR20090043450 A KR 20090043450A KR 101012089 B1 KR101012089 B1 KR 101012089B1
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- solar cell
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- 239000002096 quantum dot Substances 0.000 title claims abstract description 53
- 239000002131 composite material Substances 0.000 title claims abstract description 28
- 239000010410 layer Substances 0.000 claims abstract description 41
- 239000010409 thin film Substances 0.000 claims abstract description 34
- 239000004065 semiconductor Substances 0.000 claims abstract description 25
- 238000000034 method Methods 0.000 claims abstract description 16
- 229920000620 organic polymer Polymers 0.000 claims abstract description 14
- 239000011259 mixed solution Substances 0.000 claims abstract description 13
- 238000004519 manufacturing process Methods 0.000 claims abstract description 12
- 239000003960 organic solvent Substances 0.000 claims abstract description 10
- 239000011247 coating layer Substances 0.000 claims abstract description 9
- 238000010438 heat treatment Methods 0.000 claims abstract description 4
- 239000000758 substrate Substances 0.000 claims description 14
- 239000000203 mixture Substances 0.000 claims description 9
- UHYPYGJEEGLRJD-UHFFFAOYSA-N cadmium(2+);selenium(2-) Chemical compound [Se-2].[Cd+2] UHYPYGJEEGLRJD-UHFFFAOYSA-N 0.000 claims description 7
- 239000002245 particle Substances 0.000 claims description 6
- 239000011248 coating agent Substances 0.000 claims description 5
- 238000000576 coating method Methods 0.000 claims description 5
- 239000002105 nanoparticle Substances 0.000 claims description 5
- -1 Poly (phenylenevinylene) Polymers 0.000 claims description 4
- 150000001875 compounds Chemical class 0.000 claims description 4
- 229920003227 poly(N-vinyl carbazole) Polymers 0.000 claims description 4
- 229920000553 poly(phenylenevinylene) Polymers 0.000 claims description 4
- 238000004528 spin coating Methods 0.000 claims description 4
- GEQBRULPNIVQPP-UHFFFAOYSA-N 2-[3,5-bis(1-phenylbenzimidazol-2-yl)phenyl]-1-phenylbenzimidazole Chemical group C1=CC=CC=C1N1C2=CC=CC=C2N=C1C1=CC(C=2N(C3=CC=CC=C3N=2)C=2C=CC=CC=2)=CC(C=2N(C3=CC=CC=C3N=2)C=2C=CC=CC=2)=C1 GEQBRULPNIVQPP-UHFFFAOYSA-N 0.000 claims description 3
- DPDOFFVOHWFBEM-UHFFFAOYSA-N 1-(2-ethylhexoxy)-4-ethynylbenzene Chemical group CCCCC(CC)COC1=CC=C(C#C)C=C1 DPDOFFVOHWFBEM-UHFFFAOYSA-N 0.000 claims description 2
- STTGYIUESPWXOW-UHFFFAOYSA-N 2,9-dimethyl-4,7-diphenyl-1,10-phenanthroline Chemical compound C=12C=CC3=C(C=4C=CC=CC=4)C=C(C)N=C3C2=NC(C)=CC=1C1=CC=CC=C1 STTGYIUESPWXOW-UHFFFAOYSA-N 0.000 claims description 2
- DHDHJYNTEFLIHY-UHFFFAOYSA-N 4,7-diphenyl-1,10-phenanthroline Chemical compound C1=CC=CC=C1C1=CC=NC2=C1C=CC1=C(C=3C=CC=CC=3)C=CN=C21 DHDHJYNTEFLIHY-UHFFFAOYSA-N 0.000 claims description 2
- RXACYPFGPNTUNV-UHFFFAOYSA-N 9,9-dioctylfluorene Polymers C1=CC=C2C(CCCCCCCC)(CCCCCCCC)C3=CC=CC=C3C2=C1 RXACYPFGPNTUNV-UHFFFAOYSA-N 0.000 claims description 2
- 229910004613 CdTe Inorganic materials 0.000 claims description 2
- 229910001218 Gallium arsenide Inorganic materials 0.000 claims description 2
- 229920000109 alkoxy-substituted poly(p-phenylene vinylene) Polymers 0.000 claims description 2
- XZCJVWCMJYNSQO-UHFFFAOYSA-N butyl pbd Chemical compound C1=CC(C(C)(C)C)=CC=C1C1=NN=C(C=2C=CC(=CC=2)C=2C=CC=CC=2)O1 XZCJVWCMJYNSQO-UHFFFAOYSA-N 0.000 claims description 2
- SBIBMFFZSBJNJF-UHFFFAOYSA-N selenium;zinc Chemical compound [Se]=[Zn] SBIBMFFZSBJNJF-UHFFFAOYSA-N 0.000 claims description 2
- 238000001228 spectrum Methods 0.000 claims description 2
- 239000011229 interlayer Substances 0.000 abstract description 3
- 229910010272 inorganic material Inorganic materials 0.000 abstract 1
- 239000011147 inorganic material Substances 0.000 abstract 1
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 9
- 230000005525 hole transport Effects 0.000 description 6
- 238000010586 diagram Methods 0.000 description 4
- 239000011521 glass Substances 0.000 description 4
- 238000005259 measurement Methods 0.000 description 4
- 238000005424 photoluminescence Methods 0.000 description 4
- 229920000642 polymer Polymers 0.000 description 4
- 238000004627 transmission electron microscopy Methods 0.000 description 4
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 3
- 238000000151 deposition Methods 0.000 description 3
- 238000004770 highest occupied molecular orbital Methods 0.000 description 3
- 238000004768 lowest unoccupied molecular orbital Methods 0.000 description 3
- HEDRZPFGACZZDS-UHFFFAOYSA-N Chloroform Chemical compound ClC(Cl)Cl HEDRZPFGACZZDS-UHFFFAOYSA-N 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- AMGQUBHHOARCQH-UHFFFAOYSA-N indium;oxotin Chemical compound [In].[Sn]=O AMGQUBHHOARCQH-UHFFFAOYSA-N 0.000 description 2
- 238000004020 luminiscence type Methods 0.000 description 2
- 239000002904 solvent Substances 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 239000011258 core-shell material Substances 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 230000000593 degrading effect Effects 0.000 description 1
- 238000007606 doctor blade method Methods 0.000 description 1
- 238000005530 etching Methods 0.000 description 1
- 238000007641 inkjet printing Methods 0.000 description 1
- 230000031700 light absorption Effects 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 239000011368 organic material Substances 0.000 description 1
- 239000002356 single layer Substances 0.000 description 1
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Abstract
본 발명은 일체형 코어/쉘 구조의 고분자-양자점 복합체를 포함하는 태양전지 소자 및 이의 제조방법에 관한 것으로서, p형 유기 고분자, n형 유기 분자 및 반도체 양자점을 유기용매에 첨가하여 제조된 유-무기 혼합용액의 코팅층으로부터 가열에 의해 얻어진 일체형 코어/쉘 구조의 p-i-n 형태의 고분자-양자점 복합체 박막을 활성층으로서 이용하면 다층 박막의 층간 계면 문제를 갖지 않는 고효율 태양전지 소자를 간편하게 제조할 수 있다.The present invention relates to a solar cell device including a polymer-quantum dot composite having an integrated core / shell structure, and a method for manufacturing the same. An organic-inorganic material prepared by adding a p-type organic polymer, an n-type organic molecule, and a semiconductor quantum dot to an organic solvent. When the pin-type polymer-quantum dot composite thin film having an integral core / shell structure obtained by heating from the coating layer of the mixed solution is used as an active layer, a high efficiency solar cell device having no interlayer interface problem of the multilayer thin film can be easily manufactured.
고분자-양자점 복합체, 단일 활성층, 태양전지 Polymer-quantum dot composite, single active layer, solar cell
Description
본 발명은 일체형 코어/쉘(core/shell) 구조의 고분자-양자점 복합체로 이루어진 단일 활성층을 포함하는 태양전지 소자, 및 상기 태양전지 소자의 제조방법에 관한 것이다.The present invention relates to a solar cell device comprising a single active layer consisting of a polymer-quantum dot composite having an integral core / shell structure, and a method of manufacturing the solar cell device.
태양전지는 광전효과(photovoltaic effect)를 이용해 빛에너지를 전기에너지로 전환하는 반도체 소자로서, 햇빛이 흡수되면 전지 내부에서 전자(electron)와 정공(hole)이 생겨나고, 이 전자와 정공이 p-n 접합에 의해 생긴 전계(build-in field)를 거쳐 각각 n형 반도체(전자 수송층)와 p형 반도체(정공 수송층)로 이동하면서 공간적으로 분리된 후, 전극을 통해 내부 전자가 외부 회로로 흘러 들어가며 전류가 발생하는 원리에 근거한다.A solar cell is a semiconductor device that converts light energy into electrical energy using a photovoltaic effect. When sunlight is absorbed, electrons and holes are generated inside the cell, and the electrons and holes are pn junctions. After moving to the n-type semiconductor (electron transport layer) and p-type semiconductor (hole transport layer) through the build-in field generated by the spatially separated respectively, the internal electrons flow into the external circuit through the electrode and the current Based on the principle that arises.
최근 많이 연구되고 있는 이러한 태양전지는 일반적으로 나노입자를 이용하 는 염료감응형 태양전지, 복합구조형 태양전지 및 나노결정 박막 태양전지 등으로 구분된다.These solar cells, which have been studied recently, are generally classified into dye-sensitized solar cells, composite structure solar cells, and nanocrystalline thin film solar cells using nanoparticles.
이들 기존의 태양전지 소자는 p-n 또는 p-i-n 형태로서 대부분 정공 수송층과 전자 수송층을 포함하는 다층 박막 구조를 가지므로 (대한민국 특허공개 제2008-64438호, 제2008-77532호 및 제2008-72425호 참조), 박막을 성장하는 단계가 많아 제조비용이 높고, 다층 박막의 층간 계면(interface) 부분에 여러 가지 문제가 생겨 전지효율이 저하된다는 단점을 갖는다.These conventional solar cell devices have a multi-layered thin film structure including a hole transport layer and an electron transport layer, in the form of pn or pin (see Korean Patent Publication Nos. 2008-64438, 2008-77532, and 2008-72425). In addition, there are many stages of growing a thin film, which leads to a high manufacturing cost, and various problems occur in an interface portion of a multilayer thin film, thereby degrading battery efficiency.
따라서, 본 발명의 목적은 다층 박막 구조의 기존 태양전지 소자의 단점을 최소화하기 위해, p-i-n 형태의 고분자-양자점 복합체의 박막 형태로서 활성층을 포함하는 고효율 태양전지 소자, 및 이의 제법을 제공하는 것이다.Accordingly, an object of the present invention is to provide a high efficiency solar cell device including an active layer as a thin film form of a polymer-quantum dot composite of p-i-n type in order to minimize the disadvantages of the conventional solar cell device of a multi-layer thin film structure, and a method for manufacturing the same.
상기 목적을 달성하기 위하여 본 발명은,The present invention to achieve the above object,
기판, 양극, 활성층 및 음극이 순차적으로 적층되고, 상기 활성층으로서, p형 유기 고분자, n형 유기 분자 및 반도체 양자점을 유기용매에 첨가하여 제조된 유-무기 혼합용액의 코팅층으로부터 가열에 의해 얻어진 일체형 코어/쉘(core/shell) 구조의 p-i-n 형태의 고분자-양자점 복합체 박막을 포함하는 태양 전지 소자를 제공하는 것이다.A substrate, an anode, an active layer, and a cathode are sequentially stacked, and as the active layer, an integral type obtained by heating from a coating layer of an organic-inorganic mixed solution prepared by adding a p-type organic polymer, an n-type organic molecule, and a semiconductor quantum dot to an organic solvent. The present invention provides a solar cell device including a pin-shaped polymer-quantum dot composite thin film having a core / shell structure.
본 발명은 또한, The present invention also provides
기판 위에 양극, 활성층 및 음극이 순차적으로 적층된 태양전지 소자를 제조하는 방법에 있어서,In the method for manufacturing a solar cell device in which an anode, an active layer and a cathode are sequentially stacked on a substrate,
기판 위에 양극을 형성한 후, 상기 양극을 p형 유기 고분자, n형 유기 분자 및 반도체 양자점을 유기용매에 첨가하여 제조된 유-무기 혼합용액으로 코팅한 다음 가열하여 p-i-n 형태의 고분자-양자점 복합체의 박막 형태로서 상기 활성층을 형성하는 것을 특징으로 하는 태양전지 소자의 제조방법을 제공한다.After forming an anode on a substrate, the anode was coated with an organic-inorganic mixed solution prepared by adding a p-type organic polymer, an n-type organic molecule and a semiconductor quantum dot to an organic solvent, and then heated to obtain a pin-type polymer-quantum dot composite. It provides a method of manufacturing a solar cell device, characterized in that to form the active layer in the form of a thin film.
본 발명의 태양전지 소자 제조방법에 의하면, 양극과 음극 사이에, 일체형 코어/쉘 구조를 갖는 p-i-n 형태의 고분자-양자점 복합체의 박막 형태로서 활성층을 형성할 수 있어, 다층 박막의 층간 계면 문제를 최소화하면서 적은 비용으로 간단히 넓은 면적을 코팅할 수 있고, 낮은 온도에서도 박막을 형성할 수 있으며, 유리 기판을 비롯한 거의 모든 종류의 기판을 기판 형태의 제한 없이 다양하게 사용할 수 있다. 이와 같이 제조된 본 발명의 고효율 태양전지 소자는 구부리거나 접을 수 있어 휴대하기 편리하고, 사람의 옷, 가방, 및 휴대용 전기, 전자 제품에 부착하여 사용하기 편리하며, 빛에 대한 투명도가 높아 건물 또는 자동차의 유리창 등에 부착하여 밖을 볼 수 있게 하면서도 전력을 생산할 수 있는 등 매우 다양하게 응용될 수 있다.According to the solar cell device manufacturing method of the present invention, an active layer can be formed as a thin film of a pin-type polymer-quantum dot composite having an integrated core / shell structure between the anode and the cathode, thereby minimizing the interlayer interface problem of the multilayer thin film. While it is possible to coat a large area simply at a low cost, to form a thin film even at low temperature, almost all kinds of substrates, including glass substrates, can be used in various ways without limitation of the substrate form. The high efficiency solar cell device of the present invention manufactured as described above can be bent or folded, which is convenient to carry, and is convenient to attach to human clothes, bags, and portable electric and electronic products, and has high transparency to light or buildings. It can be applied to a wide range of applications, such as being able to produce power while being attached to a window of a car and looking outside.
본 발명에 따른 태양전지 소자는 p형 유기 고분자, n형 유기 분자 및 반도체 양자점을 유기용매에 첨가하여 제조된 유-무기 혼합용액의 코팅층으로부터 가열에 의해 얻어진 일체형 코어/쉘(core/shell) 구조의 p-i-n 형태의 고분자-양자점 복합체 박막을 활성층으로서 포함하는 것을 특징으로 한다.The solar cell device according to the present invention has an integral core / shell structure obtained by heating from a coating layer of an organic-inorganic mixed solution prepared by adding a p-type organic polymer, an n-type organic molecule, and a semiconductor quantum dot to an organic solvent. It characterized in that it comprises a pin-shaped polymer-quantum dot composite thin film as the active layer.
본 발명의 태양전지 소자 제법의 바람직한 실시양태에 따르면,According to a preferred embodiment of the solar cell device manufacturing method of the present invention,
(1) 기판(유리, 금속, 고분자, 세라믹 등) 위에 인듐-주석-산화물 (ITO, indium-tin-oxide) 박막을 증착하여 ITO 전극을 형성하고;(1) depositing an indium-tin-oxide (ITO) thin film on a substrate (glass, metal, polymer, ceramic, etc.) to form an ITO electrode;
(2) p형 유기 고분자, n형 유기 분자 및 반도체 양자점을 유기용매에 첨가하여 유-무기 혼합용액을 제조한 후, 상기 단계 (1)에서 형성된 ITO 전극을 상기 유-무기 혼합용액으로 코팅한 다음 코팅층을 가열하여 고분자-양자점 복합체 박막을 형성하고;(2) preparing an organic-inorganic mixed solution by adding a p-type organic polymer, an n-type organic molecule, and a semiconductor quantum dot to an organic solvent, and then coating the ITO electrode formed in step (1) with the organic-inorganic mixed solution. The coating layer is then heated to form a polymer-quantum dot composite thin film;
(3) 상기 단계 (2)에서 형성된 고분자-양자점 복합체 박막 위에 LiF 및 Al 박막을 순차적으로 증착하여 LiF 및 Al 전극을 형성함으로써 목적하는 태양전지 소자를 제조할 수 있다.(3) The desired solar cell device may be manufactured by sequentially depositing LiF and Al thin films on the polymer-quantum dot composite thin film formed in step (2) to form LiF and Al electrodes.
본 발명에 사용되는 p형 유기 고분자의 구체적인 예로는 폴리(N-비닐카바졸)(PVK), 폴리[1-메톡시-4-(2-에틸헥실옥시-2,5-페닐렌비닐렌)](MEH-PPV), 폴리(페닐렌비닐렌)(PPV), 디메틸페닐로 말단-캡핑된 폴리(9,9-디옥틸플루오레닐-2,7- 디일)(PFO-DMP) 및 이들의 혼합물을 들 수 있다. 이 p형 유기 고분자는 태양전지 소자에서 정공 수송층의 역할을 수행한다.Specific examples of the p-type organic polymer used in the present invention include poly (N-vinylcarbazole) (PVK), poly [1-methoxy-4- (2-ethylhexyloxy-2,5-phenylenevinylene )] (MEH-PPV), poly (phenylenevinylene) (PPV), poly (9,9-dioctylfluorenyl-2,7-diyl) (PFO-DMP) end-capped with dimethylphenyl and And mixtures thereof. This p-type organic polymer acts as a hole transport layer in the solar cell device.
본 발명에 사용되는 n형 유기 분자의 구체적인 예로는 1,3,5-트리스-(N-페닐벤즈이미다졸-2-일)벤젠(TPBi), N'-디페닐-N,N'-비스(3-메틸페닐)-1,1'-비페닐-4,4'-디아민(TPD), 2-(4-비페닐일)-5-(4-tert-부틸페닐)-1,3,4-옥사디아졸(PBD), 2,9-디메틸-4,7-디페닐-1,10-페난트롤린(BCP), 4,7-디페닐-1,10-페난트롤린(Bphen) 및 이들의 혼합물을 들 수 있다. 이 n형 유기 분자는 태양전지 소자에서 전자 수송층의 역할을 수행한다.Specific examples of n-type organic molecules used in the present invention include 1,3,5-tris- (N-phenylbenzimidazol-2-yl) benzene (TPBi), N'-diphenyl-N, N'-bis (3-methylphenyl) -1,1'-biphenyl-4,4'-diamine (TPD), 2- (4-biphenylyl) -5- (4-tert-butylphenyl) -1,3,4 -Oxadiazole (PBD), 2,9-dimethyl-4,7-diphenyl-1,10-phenanthroline (BCP), 4,7-diphenyl-1,10-phenanthroline (Bphen) and And mixtures thereof. This n-type organic molecule serves as an electron transporting layer in the solar cell device.
본 발명에 사용되는 반도체 양자점은 태양광 스펙트럼 중 200 내지 1100 nm 영역의 자외선-근적외선을 흡수하고 1.1 내지 6.0 eV 정도의 밴드갭을 갖는 반도체 나노입자로서, IV족, II족-VI족, III족-V족, I족-III족-VI족 화합물 또는 이들의 혼합물일 수 있으며, 바람직하게는 코어/쉘 구조를 갖는 II족-VI족/II족-VI족 화합물일 수 있다. 이의 구체적인 예로는 AlN(밴드갭: 6.0 eV), GaN(밴드갭: 3.4 eV), ZnO(밴드갭: 3.37 eV), InP, Si, Ge, GaAs, CuInS2, CuInSe2, CdS, CuInGaSe2, CdTe, ZnSe, CdSe/ZnS(코어/쉘) 및 이들의 혼합물을 들 수 있다. 이 반도체 양자점은 태양전지 소자에서 전기적으로 진성층(intrinsic layer)(또는 빛흡수층)의 역할을 수행한다.The semiconductor quantum dots used in the present invention are semiconductor nanoparticles that absorb ultraviolet-near infrared rays in the 200-1100 nm region of the solar spectrum and have a bandgap of about 1.1 to 6.0 eV. Group IV, Group II-VI, Group III Group-V, Group-III-VI-VI compounds or mixtures thereof, preferably Group II-VI / Group II-VI compounds having a core / shell structure. Specific examples thereof include AlN (bandgap: 6.0 eV), GaN (bandgap: 3.4 eV), ZnO (bandgap: 3.37 eV), InP, Si, Ge, GaAs, CuInS 2 , CuInSe 2 , CdS, CuInGaSe 2 , CdTe, ZnSe, CdSe / ZnS (core / shell) and mixtures thereof. This semiconductor quantum dot serves as an electrically intrinsic layer (or light absorbing layer) in the solar cell device.
본 발명에 사용되는 유기용매의 구체적인 예로는 톨루엔, 클로로포름, 디메틸포름아미드 및 이들의 혼합물을 들 수 있다.Specific examples of the organic solvent used in the present invention include toluene, chloroform, dimethylformamide and mixtures thereof.
바람직하게는, 유기용매 100 중량부에 대해 p-형 유기 고분자 0.1 ~ 10 중량부, 바람직하게는 0.6 ~ 1 중량부, n-형 유기 분자 0.1 ~ 10 중량부, 바람직하게는 0.4 ~ 1 중량부, 및 반도체 양자점 0.1 ~ 10 중량부, 바람직하게는 0.5 ~ 1 중량부를 사용할 수 있다. 이때, 최종적으로 형성되는 태양전지 소자의 전기적 특성의 조절을 위해 반도체 양자점의 사용량을 적절히 조절할 수 있다.Preferably, 0.1 to 10 parts by weight of the p-type organic polymer, preferably 0.6 to 1 part by weight, 0.1 to 10 parts by weight of the n-type organic molecule, and preferably 0.4 to 1 part by weight based on 100 parts by weight of the organic solvent. And 0.1 to 10 parts by weight, and preferably 0.5 to 1 part by weight of the semiconductor quantum dot. At this time, the amount of the semiconductor quantum dots can be appropriately adjusted to control the electrical characteristics of the finally formed solar cell device.
스핀 코팅, 잉크젯 프린팅, 롤 코팅 또는 닥터 블레이드(doctor blade)법 등을 이용하여 상기 유-무기 혼합용액으로 ITO 전극을 코팅하는데, 예를 들어 스핀 코팅의 경우 회전 속도 및 회전 시간을 조절함으로써 형성되는 코팅층, 나아가서는 고분자-양자점 복합체 박막의 두께를 정교하게 조절할 수 있다. 스핀 코팅시 회전 속도는 1000 ~ 3000 rpm으로, 회전 시간은 10 ~ 30 초로 조절할 수 있다. 코팅 두께는 0.1 ~ 10 ㎛ 일 수 있다.Coating the ITO electrode with the organic-inorganic mixed solution using spin coating, inkjet printing, roll coating or doctor blade method, for example, spin coating is formed by adjusting the rotation speed and rotation time The thickness of the coating layer, and further, the polymer-quantum dot composite thin film can be finely controlled. When spin coating, the rotation speed can be adjusted to 1000 to 3000 rpm, and the rotation time can be adjusted to 10 to 30 seconds. The coating thickness can be 0.1-10 μm.
이와 같이 형성된 코팅층을 50 내지 100℃에서 10 내지 30분 동안 가열하여 용매를 제거함으로써 ITO 전극 위에 두께 0.1 ~ 10 ㎛의 고분자-양자점 복합체 박막을 형성할 수 있다.The coating layer thus formed may be heated at 50 to 100 ° C. for 10 to 30 minutes to remove the solvent, thereby forming a polymer-quantum dot composite thin film having a thickness of 0.1 to 10 μm on the ITO electrode.
상기 단계 (1) 및 (3)에서, ITO 박막, 및 LiF 및 Al 박막은 통상적인 방법으로 증착할 수 있다.In the above steps (1) and (3), the ITO thin film, and the LiF and Al thin films can be deposited by conventional methods.
이와 같이 제조된 본 발명에 따른 태양전지 소자는 일체형 유-무기 하이브리드 입자가 개개의 독립된 p(p형 유기 고분자)-i(반도체 양자점)-n(n형 유기 분자) 형태를 갖는 고분자-양자점 복합체로 이루어진 단일 활성층을 포함한다. 이 고분자-양자점 복합체는 p-형 유기 고분자를 내부핵으로 하고, 그 고분자 입자 표면을 전기적으로 진성층(빛흡수층) 역할을 하는 반도체 양자점 나노입자들이 균일하게 둘러싸고 있으며, 또다시 그 주위를 n-형 유기 분자 입자들이 캡 형태로 둘러싸고 있는 p-i-n 형태의 일체형 코어-쉘 구조를 갖는다. 이러한 일체형 코어/쉘 구조의 고분자-양자점 복합체는 1 내지 10 nm의 입자 크기를 가질 수 있다.The solar cell device according to the present invention manufactured as described above is a polymer-quantum dot composite in which the integral organic-inorganic hybrid particles have individual independent p (p-type organic polymer) -i (semiconductor quantum dots) -n (n-type organic molecules) forms. It comprises a single active layer consisting of. This polymer-quantum dot complex has a p-type organic polymer as its inner nucleus, and is uniformly surrounded by semiconductor quantum dot nanoparticles serving as an intrinsic layer (light absorbing layer) on the surface of the polymer particle. Type organic molecular particles have a pin-shaped integral core-shell structure surrounded by a cap shape. Such monolithic core / shell structure polymer-quantum dot composite may have a particle size of 1 to 10 nm.
이러한 독립된 p-i-n 형태에서는, 정공 수송층, 진성층(빛흡수층) 및 전자 수송층이 단일층 내에 존재하게 되며, 외부에서 빛이 입사되었을 때 광전효과(photovoltaic effect)에 의해 반도체 양자점 진성층에서 광자(photon)가 흡수되어 전자-정공쌍이 생성되면 공간전하영역의 전계(build-in field)에 의해 전자와 정공이 각각 반대방향으로 흘러서 공간적으로 분리되어 전자는 전자 수송층으로, 정공은 정공 수송층으로 이동한 후 각각 전극으로 이동하게 된다. In this independent pin shape, a hole transport layer, an intrinsic layer (light absorbing layer), and an electron transport layer exist in a single layer, and photons in the intrinsic layer of the semiconductor quantum dot due to a photovoltaic effect when light is incident from the outside. When electrons are generated by the absorption of electron-hole pairs, electrons and holes flow in opposite directions by the build-in field of the space charge region, and are separated spatially, and electrons move to the electron transport layer and holes move to the hole transport layer, respectively. To the electrode.
이와 같이, 본 발명의 태양전지 소자 제조방법에 의하면, 양극과 음극 사이에, 일체형 코어/쉘 구조를 갖는 p-i-n 형태의 고분자-양자점 복합체의 박막 형태로서 활성층을 형성할 수 있어, 다층 박막의 층간 계면 문제를 최소화하면서 적은 비용으로 간단히 넓은 면적을 코팅할 수 있고, 낮은 온도에서도 박막을 형성할 수 있으며, 유리 기판을 비롯한 거의 모든 종류의 기판을 기판 형태의 제한 없이 다양하게 사용할 수 있다. 이와 같이 제조된 본 발명의 고효율 태양전지 소자는 구부리거나 접을 수 있어 휴대하기 편리하고, 사람의 옷, 가방, 및 휴대용 전기, 전자 제품에 부착하여 사용하기 편리하며, 빛에 대한 투명도가 높아 건물 또는 자동차의 유리창 등에 부착하여 밖을 볼 수 있게 하면서도 전력을 생산할 수 있는 등 매우 다양하게 응용될 수 있다.As described above, according to the solar cell device manufacturing method of the present invention, an active layer can be formed as a thin film of a pin-type polymer-quantum dot composite having an integral core / shell structure between an anode and a cathode, and thus an interlayer interface of a multilayer thin film. It is possible to coat a large area simply at a low cost while minimizing the problem, to form a thin film even at a low temperature, and almost any kind of substrate including a glass substrate can be used in various ways without limitation of the substrate form. The high efficiency solar cell device of the present invention manufactured as described above can be bent or folded, which is convenient to carry, and is convenient to attach to human clothes, bags, and portable electric and electronic products, and has high transparency to light or buildings. It can be applied to a wide range of applications, such as being able to produce power while being attached to a window of a car and looking outside.
이하, 본 발명을 하기 실시예에 의거하여 좀더 상세하게 설명하고자 한다. 단, 하기 실시예는 본 발명을 예시하기 위한 것일 뿐, 본 발명의 범위가 이들만으로 제한되는 것은 아니다.Hereinafter, the present invention will be described in more detail based on the following examples. However, the following examples are only for illustrating the present invention, and the scope of the present invention is not limited thereto.
[실시예 1]Example 1
유리 기판 위에 인듐-주석-산화물 (ITO, indium-tin-oxide) 박막을 증착한 후 식각 공정을 거쳐 종방향과 같은 형태의 ITO 전극을 형성하였다. 폴리(N-비닐카바졸)(PVK)(중량평균분자량: 25,000 내지 50,000), 1,3,5-트리스-(N-페닐벤즈이미다졸-2-일)벤젠(TPBi) 및 코어/쉘 구조의 CdSe/ZnS 양자점을 톨루엔에 첨가하여 유-무기 혼합용액을 제조하였다. 이때, 톨루엔 100 중량부에 대해 PVK, TPBi 및 CdSe/ZnS 양자점을 각각 0.5 중량부, 0.6 중량부 및 0.4 중량부의 양으로 사용하였다.After depositing an indium-tin-oxide (ITO) thin film on a glass substrate, an ITO electrode was formed in the longitudinal direction through an etching process. Poly (N-vinylcarbazole) (PVK) (weight average molecular weight: 25,000 to 50,000), 1,3,5-tris- (N-phenylbenzimidazol-2-yl) benzene (TPBi) and core / shell structure CdSe / ZnS quantum dots of to was added to toluene to prepare an organic-inorganic mixed solution. At this time, PVK, TPBi and CdSe / ZnS quantum dots were used in an amount of 0.5 parts by weight, 0.6 parts by weight and 0.4 parts by weight based on 100 parts by weight of toluene, respectively.
상기 유-무기 혼합용액으로 ITO 전극을 스핀 코팅하였으며, 스핀 코팅시 회전 속도는 2000 rpm으로, 회전 시간은 20 초로 조절하였다. 이와 같이 형성된 코팅층을 약 100℃에서 약 10분 동안 가열하여 용매를 제거함으로써 ITO 전극 위에 두께 150 nm의 단일 활성층으로서의 고분자-양자점 복합체 박막을 형성하였다.The ITO electrode was spin-coated with the organic-inorganic mixed solution, and the spin speed was adjusted to 2000 rpm and the spin time was 20 seconds. The coating layer thus formed was heated at about 100 ° C. for about 10 minutes to remove the solvent to form a polymer-quantum dot composite thin film as a single active layer having a thickness of 150 nm on the ITO electrode.
이어, 형성된 고분자-양자점 복합체 박막 위에, 열 증류기(thermal evaporator)를 사용하여 LiF 및 Al 박막을 순차적으로 증착하여 횡방향으로 LiF 및 Al 전극을 형성한 후, 형성된 적층체에 대해서 구동 회로를 형성하여 목적하는 태양전지 소자를 제조하였다.Subsequently, LiF and Al thin films are sequentially deposited on the formed polymer-quantum dot composite thin film using a thermal evaporator to form LiF and Al electrodes in the transverse direction, and then a driving circuit is formed for the formed laminate. The desired solar cell device was manufactured.
상기 실시예 1에서 제조된, 일체형 코어/쉘 구조를 갖는 p-i-n 형태의 고분자-양자점 복합체의 박막을 단일 활성층으로서 포함하는 태양전지 소자의 단면도를 도 1에 나타내었다. 1 is a cross-sectional view of a solar cell device including a thin film of p-i-n type polymer-quantum dot composite having an integrated core / shell structure as a single active layer prepared in Example 1.
상기 실시예 1에서 얻어진 코어/쉘 구조의 고분자-양자점 복합체의 투과전자현미경(transmission electron microscopy, TEM) 사진을 도 2에 나타내었다. 도 2로부터, 100-200 nm 크기의 PVK 고분자 표면에 수 nm 크기의 양자점이 흡착되어 있는 것처럼 분포하고 있으며, PVK와 양자점 전체를 TPBi 저분자 유기물이 감싸는 것을 확인할 수 있고, 이로 인해 p(PVK)-i(CdSe/ZnS)-n(TPBi) 구조가 형성되어 있음을 최초로 확인하였다.A transmission electron microscopy (TEM) photograph of the polymer-quantum dot composite having a core / shell structure obtained in Example 1 is shown in FIG. 2. From FIG. 2, it can be seen that quantum dots of several nm size are distributed on the surface of 100-200 nm PVK polymer, and TPBi low molecular weight organic material is wrapped around PVK and the quantum dots, thereby p (PVK)- It was confirmed for the first time that the i (CdSe / ZnS) -n (TPBi) structure was formed.
도 2의 TEM 사진을 기초로 하여 상기 실시예 1에서 제조된 태양전지 소자의 모식도를 도 3에 나타내었다. 도 3으로부터, Al 전극과 ITO 전극 양단 사이에, TPBi (n형 전자 수송층)가 PVK 고분자 (p형 정공 수송층)를 감싸고 그 사이 진성층으로서 CdSe/ZnS 양자점 나노입자가 형성되어 빛이 입사할 때 빛을 흡수하는 등 p-i-n 형태의 층이 형성되었음을 알 수 있다.A schematic diagram of the solar cell device manufactured in Example 1 based on the TEM photograph of FIG. 2 is shown in FIG. 3. From Fig. 3, when TPBi (n-type electron transport layer) surrounds PVK polymer (p-type hole transport layer) between the Al electrode and the ITO electrode, CdSe / ZnS quantum dot nanoparticles are formed as the intrinsic layer therebetween, and the light is incident. It can be seen that a pin-like layer is formed to absorb light.
상기 실시예 1에서 제조된 태양전지 소자의 전류밀도-전압 (J-V) 측정 곡선을 도 4에 나타내었다. 이때, 태양광 시뮬레이터(solar simulator) 장치를 사용하 여 태양 빛을 입사시켜 측정하였다. 도 4로부터, 처음 시작점의 전류밀도가 태양 빛의 입사를 통해 전자와 정공이 전극을 통해 들어가면서 커지다가 시간이 지남에 따라 전압 1.2 V 근처에서 감소하는 것을 알 수 있다. A current density-voltage (J-V) measurement curve of the solar cell device manufactured in Example 1 is shown in FIG. 4. In this case, the solar light was measured by using a solar simulator device. From FIG. 4, it can be seen that the current density of the initial starting point increases as electrons and holes enter through the electrode through the incidence of solar light, and then decreases around 1.2 V with time.
상기 실시예 1에서 제조된 태양전지 소자의 에너지 밴드 다이어그램을 도 5에 나타내었다. 도 5로부터, 빛의 흡수를 통해서 전자와 정공이 나뉘어져 서로 각각 다르게 이동함을 알 수 있다. 전자의 구체적인 이동 경로를 살펴보면, 전자는 TPBi LUMO (the lowest unoccupied molecular orbital) 레벨까지 호핑 메카니즘(hopping machanism)을 통하여 이동한 후 TPBi LUMO 레벨에서 다음 단계인 Al 전극으로 이동한다. 반대편에 있는 정공의 이동 경로를 살펴보면, 정공은 PVK HOMO (the highest occupied molecular orbital) 레벨로 이동한 후 PVK HOMO 레벨에서 다음 단계인 ITO 투명전극으로 이동하여 기전력을 발생시켜 전류를 흐르게 한다. An energy band diagram of the solar cell device manufactured in Example 1 is illustrated in FIG. 5. 5, it can be seen that electrons and holes are divided and moved differently through absorption of light. Looking at the specific path of the electron, the electron moves through the hopping mechanism (hopping machanism) to the lowest unoccupied molecular orbital (TPBi LUMO) level, and then to the Al electrode of the next step at the TPBi LUMO level. Looking at the movement path of the hole on the opposite side, the hole moves to the highest occupied molecular orbital (PVK HOMO) level, and then moves to the next step, the ITO transparent electrode, at the PVK HOMO level to generate electromotive force to flow the current.
상기 실시예 1에서 제조된 태양전지 소자의 광발광 (photoluminescence, PL) 측정 곡선을 도 6에 나타내었다. 도 6의 곡선에서, PVK 및 TPBi 입자로부터의 발광은 400-500 nm 영역에 걸쳐 관찰되었고, CdSe 반도체 양자점으로부터의 발광은 585 nm 근처에서 오렌지색 발광이 관측되었다. A photoluminescence (PL) measurement curve of the solar cell device manufactured in Example 1 is shown in FIG. 6. In the curve of FIG. 6, luminescence from PVK and TPBi particles was observed over the 400-500 nm region, and luminescence from the CdSe semiconductor quantum dots was observed at around 585 nm.
도 1은 상기 실시예 1에서 제조된, 일체형 코어/쉘 구조를 갖는 p-i-n 형태의 고분자-양자점 복합체의 박막을 단일 활성층으로서 포함하는 태양전지 소자의 단면도이고,1 is a cross-sectional view of a solar cell device including a thin film of a polymer-quantum dot composite of p-i-n type having an integrated core / shell structure prepared in Example 1 as a single active layer,
도 2는 상기 실시예 1에서 얻어진 코어/쉘 구조의 고분자-양자점 복합체의 투과전자현미경(TEM) 사진이고,2 is a transmission electron microscope (TEM) photograph of a polymer-quantum dot composite having a core / shell structure obtained in Example 1,
도 3은 도 2의 TEM 사진을 기초로 하여 상기 실시예 1에서 제조된 태양전지 소자의 모식도이고,FIG. 3 is a schematic diagram of the solar cell device manufactured in Example 1 based on the TEM photograph of FIG. 2.
도 4는 상기 실시예 1에서 제조된 태양전지 소자의 전류밀도-전압 (J-V) 측정 곡선이고,4 is a current density-voltage (J-V) measurement curve of the solar cell device manufactured in Example 1,
도 5는 상기 실시예 1에서 제조된 태양전지 소자의 에너지 밴드 다이어그램이고,5 is an energy band diagram of the solar cell device manufactured in Example 1,
도 6은 상기 실시예 1에서 제조된 태양전지 소자의 광발광 (PL) 측정 곡선이다. 6 is a photoluminescence (PL) measurement curve of the solar cell device manufactured in Example 1.
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| KR101351336B1 (en) | 2011-10-07 | 2014-01-16 | 한국과학기술연구원 | Metal oxide Semiconductor-Nanocarbon Consolidated Core-shell Quantum dots and Ultraviolet Photovoltaic Cell using it and A fabrication process thereof |
| KR20190085251A (en) * | 2018-01-10 | 2019-07-18 | 세종대학교산학협력단 | Inorganic hybrid photonic film and method of preparing the same |
| KR102172248B1 (en) | 2018-01-10 | 2020-10-30 | 세종대학교산학협력단 | Inorganic hybrid photonic film and method of preparing the same |
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| US20100294355A1 (en) | 2010-11-25 |
| KR20100124446A (en) | 2010-11-29 |
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